Sn nanopillar arrays embedded between graphene sheets were assembled using a conventional film deposition and annealing process. The as-formed three-dimensional (3D) multilayered nanostructure was directly used as an anode material for rechargeable lithium-ion batteries without adding any polymer binder and carbon black. Electrochemical measurements showed very high reversible capacity and excellent cycling performance at a current density as high as 5 A g−1. These results demonstrated that nanocomposite materials with highly functional 1D and 2D components can be synthesized by employing conventional top-down manufacturing methods and self-assembly principles.